Alteration Behavior of High Burnup Spent Fuel in Salt Brine Under Hydrogen Overpressure and in Presence of Bromide

Recent studies have shown that in the presence of H2 overpressure, which forms due to the corrosion of the Fe based container, the dissolution rate of the spent fuel matrix is slowed down by a factor of about 10, associated with a distinct decrease of concentrations of important radionuclides. However, in a natural salt environment as well as in geological formations with chloride rich groundwater the presence of radiation chemically active impurities such as bromide must be taken in consideration. Bromide is known to react with {beta}/{gamma} radiolysis products, thus counteracting the protective H{sub 2} effect. In the present experiments using high burnup spent fuel, it is observed that during 212 days the matrix dissolution rate was enhanced by a factor of about 10 in the presence of up to 10{sup -3} M bromide and 3.2 bar H{sub 2} overpressure. However, concentrations of matrix bound actinides were found at the same level or below as found under identical conditions, but in the absence of bromide. In the long-term it is expected that the effect of bromide becomes less important, because the decrease of {beta}/{gamma}-activity results in a decrease of oxidative radicals, which react with bromide, while a-activity will dominate themore » radiation field. (authors)« less